In the art of making silicon nitride, it is conventional to add certain oxides to the raw material from which the fully dense silicon nitride body is constituted, such oxides act as pressing aids or sintering aids (see U.S. Pat. No. 4,143,107). The presence of these oxides has required higher temperatures, pressures, and pressing times to reach full densification, during hot pressing or sintering, than what is optimally desired for a more economical process.
Generally, compounds other than oxides have been introduced to silicon nitride as a result of chemical reaction during hot pressing or sintering (see U.S. Pat. Nos. 4,102,698; 4,341,874; and 4,350,771). Rarely have compounds other than oxides been introduced to Si.sub.3 N.sub.4 prior to hot pressing or sintering. One indirect instance is disclosed in copending U.S. application Ser. No. 444,251, PCT application No. 82/01372, commonly assigned to the assignee of this invention. In this latter case, oxides were added to a silicon metal mixture and the mixture was nitrided to react the oxides and form a composite of silicon nitride, oxynitrides, and a small amount of silicate. Under this disclosure, the nitriding step was not able to optimally fulfill the dual roles imposed upon it, that is: (a) to efficiently convert all of the silicon to silicon nitride, and (b) at the same time form only a selected silicon oxynitride in a controlled optimum amount.
What is needed is the ability to introduce chemical modifications to the mixture prior to nitriding or heat treatment, which modifications allow for: (a) a more efficient conversion of silicon to silicon nitride, (b) a reduction in the time and temperature required in subsequent steps to hot press or sinter the mixture to a fully densified object, (c) freedom to decrease the amount of silicate forming oxide to a much lower controlled amount to optimize physical characteristics in the final object, and (d) closer control and proportioning of the desired secondary phase chemistry in the final product without total reliance on the vagaries of chemical reaction during any reaction heating involved in the process such as during nitriding, hot pressing, or sintering.
Continuing research, as exemplified herein, underscores the need for selectivity of silicon oxynitrides and the need for greater silicon conversion efficiency. Certain of these oxynitrides are more desirable than others and more desirable than silicates or oxides in promoting lower temperatures and pressures needed for processing. This selectivity is due in part to the fact that certain of these compounds have a higher degree of solubility for silicon nitride, thus tending to promote a reduction in at least one of the processing parameters (temperature, pressure, or hot pressing time) needed for full dissolution of the silicon nitride during the heat fusion step.